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Title: Ion transport and softening in a polymerized ionic liquid

Abstract

Polymerized ionic liquids (PolyILs) are promising materials for various solid state electronic applications such as dye-sensitized solar cells, lithium batteries, actuators, field-effect transistors, light emitting electrochemical cells, and electrochromic devices. However, fundamental understanding of interconnection between ionic transport and mechanical properties in PolyILs is far from complete. In this paper, local charge transport and structural changes in films of a PolyIL are studied using an integrated experiment-theory based approach. Experimental data for the kinetics of charging and steady state current–voltage relations can be explained by taking into account the dissociation of ions under an applied electric field (known as the Wien effect). Onsager's theory of the Wien effect coupled with the Poisson–Nernst–Planck formalism for the charge transport is found to be in excellent agreement with the experimental results. The agreement between the theory and experiments allows us to predict structural properties of the PolyIL films. We have observed significant softening of the PolyIL films beyond certain threshold voltages and formation of holes under a scanning probe microscopy (SPM) tip, through which an electric field was applied. Finally, the observed softening is explained by the theory of depression in glass transition temperature resulting from enhanced dissociation of ions with an increasemore » in applied electric field.« less

Authors:
 [1];  [2];  [3];  [3];  [3];  [4];  [4];  [2];  [5];  [5];  [6];  [7];  [3];  [1]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computer Science and Mathematics Division; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
  4. Hochschule Niederrhein Univ. of Applied Sciences, Krefeld (Germany). Dept. of Chemistry. Inst. for Coatings and Surface Chemistry
  5. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering
  6. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1286714
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 7; Journal Issue: 3; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kumar, Rajeev, Bocharova, Vera, Strelcov, Evgheni, Tselev, Alexander, Kravchenko, Ivan I., Berdzinski, Stefan, Strehmel, Veronika, Ovchinnikova, Olga S., Minutolo, Joseph A., Sangoro, Joshua R., Agapov, Alexander L., Sokolov, Alexei P., Kalinin, Sergei V., and Sumpter, Bobby G. Ion transport and softening in a polymerized ionic liquid. United States: N. p., 2014. Web. doi:10.1039/C4NR05491A.
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Kumar, Rajeev, Bocharova, Vera, Strelcov, Evgheni, Tselev, Alexander, Kravchenko, Ivan I., Berdzinski, Stefan, Strehmel, Veronika, Ovchinnikova, Olga S., Minutolo, Joseph A., Sangoro, Joshua R., Agapov, Alexander L., Sokolov, Alexei P., Kalinin, Sergei V., & Sumpter, Bobby G. Ion transport and softening in a polymerized ionic liquid. United States. https://doi.org/10.1039/C4NR05491A
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Kumar, Rajeev, Bocharova, Vera, Strelcov, Evgheni, Tselev, Alexander, Kravchenko, Ivan I., Berdzinski, Stefan, Strehmel, Veronika, Ovchinnikova, Olga S., Minutolo, Joseph A., Sangoro, Joshua R., Agapov, Alexander L., Sokolov, Alexei P., Kalinin, Sergei V., and Sumpter, Bobby G. Thu . "Ion transport and softening in a polymerized ionic liquid". United States. https://doi.org/10.1039/C4NR05491A. https://www.osti.gov/servlets/purl/1286714.
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@article{osti_1286714,
title = {Ion transport and softening in a polymerized ionic liquid},
author = {Kumar, Rajeev and Bocharova, Vera and Strelcov, Evgheni and Tselev, Alexander and Kravchenko, Ivan I. and Berdzinski, Stefan and Strehmel, Veronika and Ovchinnikova, Olga S. and Minutolo, Joseph A. and Sangoro, Joshua R. and Agapov, Alexander L. and Sokolov, Alexei P. and Kalinin, Sergei V. and Sumpter, Bobby G.},
abstractNote = {Polymerized ionic liquids (PolyILs) are promising materials for various solid state electronic applications such as dye-sensitized solar cells, lithium batteries, actuators, field-effect transistors, light emitting electrochemical cells, and electrochromic devices. However, fundamental understanding of interconnection between ionic transport and mechanical properties in PolyILs is far from complete. In this paper, local charge transport and structural changes in films of a PolyIL are studied using an integrated experiment-theory based approach. Experimental data for the kinetics of charging and steady state current–voltage relations can be explained by taking into account the dissociation of ions under an applied electric field (known as the Wien effect). Onsager's theory of the Wien effect coupled with the Poisson–Nernst–Planck formalism for the charge transport is found to be in excellent agreement with the experimental results. The agreement between the theory and experiments allows us to predict structural properties of the PolyIL films. We have observed significant softening of the PolyIL films beyond certain threshold voltages and formation of holes under a scanning probe microscopy (SPM) tip, through which an electric field was applied. Finally, the observed softening is explained by the theory of depression in glass transition temperature resulting from enhanced dissociation of ions with an increase in applied electric field.},
doi = {10.1039/C4NR05491A},
journal = {Nanoscale},
number = 3,
volume = 7,
place = {United States},
year = {Thu Nov 13 00:00:00 EST 2014},
month = {Thu Nov 13 00:00:00 EST 2014}
}
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https://doi.org/10.1039/C4NR05491A
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